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Ionic liquid based mixtures for gas storage and delivery

a technology of ionic liquid and gas storage, which is applied in the direction of liquid degasification, separation process, and other chemical processes, can solve the problems of toxic gas storage under high pressure in metal cylinders, gas safety and environmental challenges, and inability to meet the needs of storage and delivery systems, etc., and achieve the effect of reducing the solubility of unreacted gas

Inactive Publication Date: 2009-07-21
VERSUM MATERIALS US LLC
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0008]In yet another aspect, there is provided a method method for the removal of at least a portion of an unreacted gas from a mixture comprising a chemically reacted gas, an ionic liquid, and the unreacted gas comprising: providing the ionic liquid comprising an anion and a cation within a storage vessel; introducing the unreacted gas to the storage vessel comprising the ionic liquid wherein at least a portion of the unreacted gas resides within a headspace of the storage vessel; reacting at least a portion of a gas selected from the group consisting of a boron-containing gas, an aluminum-containing gas, a phosphorous-containing gas, an arsenic-containing gas, an ether-containing gas, a nitrogen-containing gas, an antimony-containing gas, a bismuth-containing gas, a selenium-containing gas, a gallium-containing gas, a silicon-containing gas, a germanium-containing gas, a tin-containing gas, a tellurium-containing gas, a halogen-containing gas, a halocarbonyl-containing gas, an oxygen-containing gas and mixtures thereof with the ionic liquid to provide the mixture comprising the ionic liquid, a chemically reacted gas disposed within the ionic liquid, and the unreacted gas; reducing the temperature of the mixture to solidify the ionic liquid and provide a solidified mixture comprising the ionic liquid and chemically reacted gas wherein the reducing decreases the solubility of the unreacted gas thereby causing the unreacted gas to evolve into the headspace; removing substantially all of the unreacted gas from the headspace; and increasing the temperature of solidified mixture to provide a mixture substantially free of unreacted gas.

Problems solved by technology

These gases pose significant safety and environmental challenges due to their high toxicity and pyrophoricity (spontaneous flammability in air).
In addition to the toxicity factor, many of these gases are compressed and liquefied for storage in cylinders under high pressure.
Storage of toxic gases under high pressure in metal cylinders is often unacceptable because of the possibility of developing a leak or catastrophic rupture of the cylinder.
These storage and delivery systems are not without their problems.
They suffer from poor capacity and delivery limitations, poor thermal conductivity, and so forth.

Method used

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  • Ionic liquid based mixtures for gas storage and delivery

Examples

Experimental program
Comparison scheme
Effect test

example 1

Mixture Formed from Reaction of Lewis Acidic Ionic Liquid BMIM+Al2Cl7− and PH3

[0068]Molecular modeling was used to calculate a binding energy, ΔErxn, for this Lewis acidic ionic liquid with PH3. The ionic liquid was modeled as an ion-pair, using 1,3-dimethylimidazolium as the cation, Al2Cl7− as the anion, and it was assumed that one equivalent of PH3 reacted per equivalent of Al2Cl7− anion (concentration of Al2Cl7−=3.2 mol / L). Structures were determined based on minimum energy geometry optimization using Density Functional Theory (DFT) at the BP level with a double numerical (DN**) basis set. This Lewis acidic ionic liquid was calculated to have a ΔErxn of 0.71 kcal / mol, which suggests that the reaction is slightly unfavorable, although within the general limitations of error. To clarify the results of modeling, the following reaction was run.

[0069]In a glove box, 9.07 g of AlCl3 (2 equivalents) was slowly added to 5.94 g (1 equivalent) of 1-butyl-3-methylimidazolium chloride (BMIM...

example 2

Mixture Formed from Reaction of Lewis Acidic Ionic Liquid BMIM+CuCl2− and PH3

[0072]In a glove box, 3.10 g of CuCl was slowly added to a flask charged with 5.46 g of BMIM+Cl− (1:1 stoichiometry) (assuming the anion CuCl2− is formed from the reaction stoichiometry 1 equivalent CuCl to 1 equivalent BMIM+Cl−). The mixture was stirred overnight and stored. A glass insert was charged with 7.71 g of the ionic liquid (density=1.4 g / mL) and placed into a 50 mL reactor, and the general procedure for measuring PH3 reaction was followed. The Lewis acidic ionic liquid reacted with 7.6 mmol of PH3 at room temperature and 674 Torr, corresponding to 1.4 mol PH3 / L of ionic liquid. Equilibrium data points were not obtained and % reversibility and working capacity were not determined.

example 3

Mixture Formed from Reaction of Lewis Acidic Ionic Liquid BMIM+Cu2Cl3− and PH3

[0073]Molecular modeling was used to approximate the effectiveness of BMIM+Cu2Cl3− as a reactive liquid. The ionic liquid was modeled as an ion-pair, using 1,3-dimethylimidazolium as the cation, Cu2Cl3− as the anion, and it was assumed that one equivalent of PH3 reacted with each equivalent of copper (concentration of Cu reactive groups=9.7 mol / L). Structures were determined based on minimum energy geometry optimization using Density Functional Theory (DFT) at the BP level with a double numerical (DN**) basis set. This Lewis acidic ionic liquid was calculated to have an average ΔErxn of −5.5 kcal / mol for its reaction with PH3. The results indicate that this ionic liquid should bind PH3 more strongly than BMIM+Al2Cl7− of Example 1. Since ΔGrxn is smaller in magnitude than ΔErxn and the optimum ΔGrxn for the pressure range 20 to 760 Torr at room temperature is ca. −3 kcal / mol, the result suggests that the ...

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Abstract

A mixture and method for the storage and delivery of a gas are disclosed herein. In one aspect, there is provided a mixture comprising: an ionic liquid comprising an anion and a cation, at least a portion of the gas that is disposed within and reversibly chemically reacted with the ionic liquid, and optionally an unreacted gas. In another aspect, there is provided a method for delivering a gas from a mixture comprising an ionic liquid and one or more gases comprising: reacting at least a portion of the gas with the ionic liquid to provide the mixture comprising a chemically reacted gas and an ionic liquid and separating the chemically reacted gas from the mixture wherein the chemically reacted gas after the separating step has substantially the same chemical identity as the chemically reacted gas prior to the reacting step.

Description

CROSS-REFERENCE TO RELATED APPLICATIONS[0001]This application is a continuation-in-part of U.S. patent application Ser. No. 10 / 948,277, filed 23 Sep. 2004, the disclosure of which is incorporated herein by reference in its entirety.BACKGROUND OF THE INVENTION[0002]Many processes in the semiconductor industry require a reliable source of process gases for a wide variety of applications. Often these gases are stored in cylinders or vessels and then delivered to the process under controlled conditions from the cylinder. The semiconductor manufacturing industry, for example, uses a number of hazardous specialty gases such as phosphine (PH3), arsine (AsH3), and boron trifluoride (BF3) for doping, etching, and thin-film deposition. These gases pose significant safety and environmental challenges due to their high toxicity and pyrophoricity (spontaneous flammability in air). In addition to the toxicity factor, many of these gases are compressed and liquefied for storage in cylinders under ...

Claims

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Application Information

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Patent Type & Authority Patents(United States)
IPC IPC(8): B01D19/00F17C11/00
CPCC01B3/001C01B9/08C01B13/0285C01B25/06F17C11/00F17C11/005F17C11/007C01B31/28Y02E60/324Y02E60/321C01B32/80Y02E60/32
Inventor TEMPEL, DANIEL JOSEPHHENDERSON, PHILIP BRUCEBRZOZOWSKI, JEFFREY RICHARDPEARLSTEIN, RONALD MARTINGARG, DIWAKAR
Owner VERSUM MATERIALS US LLC
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